Nanomaterials2014, 4(1), 129-154; doi:10.3390/nano4010129 - published online 6 February 2014 Show/Hide Abstract
Abstract: Lanthanide-doped upconversion-luminescent nanoparticles (UCNPs), which can be excited by near-infrared (NIR) laser irradiation to emit multiplex light, have been proven to be very useful for in vitro and in vivo molecular imaging studies. In comparison with the conventionally used down-conversion fluorescence imaging strategies, the NIR light excited luminescence of UCNPs displays high photostability, low cytotoxicity, little background auto-fluorescence, which allows for deep tissue penetration, making them attractive as contrast agents for biomedical imaging applications. In this review, we will mainly focus on the latest development of a new type of lanthanide-doped UCNP material and its main applications for in vitro and in vivo molecular imaging and we will also discuss the challenges and future perspectives.
Nanomaterials2014, 4(1), 87-128; doi:10.3390/nano4010087 - published online 29 January 2014 Show/Hide Abstract
Abstract: This paper reviews the current progress in mathematical modeling of anti-reflective subwavelength structures. Methods covered include effective medium theory (EMT), finite-difference time-domain (FDTD), transfer matrix method (TMM), the Fourier modal method (FMM)/rigorous coupled-wave analysis (RCWA) and the finite element method (FEM). Time-based solutions to Maxwell’s equations, such as FDTD, have the benefits of calculating reflectance for multiple wavelengths of light per simulation, but are computationally intensive. Space-discretized methods such as FDTD and FEM output field strength results over the whole geometry and are capable of modeling arbitrary shapes. Frequency-based solutions such as RCWA/FMM and FEM model one wavelength per simulation and are thus able to handle dispersion for regular geometries. Analytical approaches such as TMM are appropriate for very simple thin films. Initial disadvantages such as neglect of dispersion (FDTD), inaccuracy in TM polarization (RCWA), inability to model aperiodic gratings (RCWA), and inaccuracy with metallic materials (FDTD) have been overcome by most modern software. All rigorous numerical methods have accurately predicted the broadband reflection of ideal, graded-index anti-reflective subwavelength structures; ideal structures are tapered nanostructures with periods smaller than the wavelengths of light of interest and lengths that are at least a large portion of the wavelengths considered.
Nanomaterials2014, 4(1), 69-86; doi:10.3390/nano4010069 - published online 8 January 2014 Show/Hide Abstract
Abstract: We report a one-pot solvothermal synthesis of sub-10 nm, dominant ultraviolet (UV) emissive upconverting nanocrystals (UCNCs), based on sodium-codoped LaF3 and BaLaF5 (0.5%Tm; 20%Yb) and their corresponding core@shell derivatives. Elemental analysis shows a Na-codopant in these crystal systems of ~20% the total cation content; X-ray diffraction (XRD) data indicate a shift in unit cell dimensions consistent with these small codopant ions. Similarly, X-ray photoelectron spectroscopic (XPS) analysis reveals primarily substitution of Na+ for La3+ ions (97% of total Na+ codopant) in the crystal system, and interstitial Na+ (3% of detected Na+) and La3+ (3% of detected La3+) present in (Na)LaF3 and only direct substitution of Na+ for Ba2+ in Ba(Na)LaF5. In each case, XPS analysis of La 3d lines show a decrease in binding energy (0.08–0.25 eV) indicating a reduction in local crystal field symmetry surrounding rare earth (R.E.3+) ions, permitting otherwise disallowed R.E. UC transitions to be enhanced. Studies that examine the impact of laser excitation power upon luminescence intensity were conducted over 2.5–100 W/cm2 range to elucidate UC mechanisms that populate dominant UV emitting states. Low power saturation of Tm3+3F3 and 3H4 states was observed and noted as a key initial condition for effective population of the 1D2 and 1I6 UV emitting states, via Tm-Tm cross-relaxation.
Nanomaterials2014, 4(1), 55-68; doi:10.3390/nano4010055 - published online 3 January 2014 Show/Hide Abstract
Abstract: The luminescence efficiency of lanthanide-doped upconversion nanoparticles is of particular importance for their embodiment in biophotonic and photonic applications. Here, we show that the upconversion luminescence of typically used NaYF4:Yb3+30%/Tm3+0.5% nanoparticles can be enhanced by ~240 times through a hierarchical active core/active shell/inert shell (NaYF4:Yb3+30%/Tm3+0.5%)/NaYbF4/NaYF4 design, which involves the use of directed energy migration in the second active shell layer. The resulting active core/active shell/inert shell nanoparticles are determined to be about 11 times brighter than that of well-investigated (NaYF4:Yb3+30%/Tm3+0.5%)/NaYF4 active core/inert shell nanoparticles when excited at ~980 nm. The strategy for enhanced upconversion in Yb3+/Tm3+-codoped NaYF4 nanoparticles through directed energy migration might have implications for other types of lanthanide-doped upconversion nanoparticles.
Nanomaterials2014, 4(1), 46-54; doi:10.3390/nano4010046 - published online 2 January 2014 Show/Hide Abstract
Abstract: In this investigation, the low-frequency alternate-current (AC) magnetic susceptibility (χac) and hysteresis loop of various MgO thickness in CoFeB/MgO/CoFeB magnetic tunneling junction (MTJ) determined coercivity (Hc) and magnetization (Ms) and correlated that with χac maxima. The multilayer films were sputtered onto glass substrates and the thickness of intermediate barrier MgO layer was varied from 6 to 15 Å. An experiment was also performed to examine the variation of the highest χac and maximum phase angle (θmax) at the optimal resonance frequency (fres), at which the spin sensitivity is maximal. The results reveal that χac falls as the frequency increases due to the relationship between magnetization and thickness of the barrier layer. The maximum χac is at 10 Hz that is related to the maximal spin sensitivity and that this corresponds to a MgO layer of 11 Å. This result also suggests that the spin sensitivity is related to both highest χac and maximum phase angle. The corresponding maximum of χac is related to high exchange coupling. High coercivity and saturation magnetization contribute to high exchange-coupling χac strength.